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Visible-light-induced controllable transformations of cumulative aryldienes through an energy transfer process

Science China Chemistry 2025年第3期68卷 987-1001页

作者： Ling Qian Ziqi Yu Jiaxin Liu Yin Wei Min Shi Key Laboratory for Advanced Materials and Institute of Fine Chemicals Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry&Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisUniversity of Chinese Academy of SciencesShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Key Laboratory of Fluorine and Nitrogen Chemistry and Advanced Materials Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032China

In this work,we report a visible light-induced energy transfer process related photochemical protocol of cumulative diene containing compounds for the construction of benzocyclohexene skeletons or the corresponding aromatized structures through an energy transfer process,1,5-hydrogen atom transfer and a 6πelectrocyclization or demethoxylation in the presence of different photocatalysts such as[Ir(dF(Me)ppy)_(2)(dtbbpy)]PF_(6) or *** newly developed photochemical strategy is characterized by mild conditions,broad substrate applicability,good functional group tolerance and good *** mechanistic paradigm was clarified by deuterium labeling,kinetic,photophysical and electrochemical analyses,control experiments and density functional theory(DFT)*** transformation of the obtained product to the drug-like molecules such as Sertraline and the luminescent conjugated aromatic compounds has also been disclosed.

关键词： visible-light photocatalysis EnT process 1,5-HAT remote C(sp^(3))-H bond activation

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Rational design and synthesis of Cr_(1-x)Te/Ag_(2)Te composites for solid-state thermoelectromagnetic cooling near room temperature

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Chinese Physics B 2024年第5期33卷 580-586页

作者：孙笑晨谢承昊陈思汗万京伟谭刚健唐新峰 State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China International School of Materials Science & Engineering Wuhan University of TechnologyWuhan 430070China

materials with both large magnetocaloric response and high thermoelectric performance are of vital importance for all-solid-state thermoelectromagnetic *** two properties,however,hardly coexist in single phase materials except previously reported hexagonal Cr_(1-x)Te half metal where a relatively high magnetic entropy change(-△S_(M))of~2.4 J·kg^(-1)·K^(-1)@5 T and a moderate thermoelectric figure of merit(ZT)of~1.2×10^(-2)@300 K are simultaneously *** we aim to increase the thermoelectric performance of Cr_(1-x)Te by compositing with semiconducting Ag_(2)*** is discovered that the in-situ synthesis of Cr_(1-x)Te/Ag_(2)Te composites by reacting their constitute elements above melting temperatures is unsuccessful because of strong phase ***,at elevated temperatures(T>800 K),Cr_(1-x)Te has a much lower deformation energy than Ag_(2)Te and tends to become more Cr-deficient by capturing Te from Ag_(2)***,Ag is insufficiently reacted and as a metal it deteriorates *** then rationalize the synthesis of Cr_(1-x)Te/Ag_(2)Te composites by ex-situ mix of the pre-prepared Cr_(1-x)Te and Ag_(2)Te binary compounds followed by densification at a low sintering temperature of 573 K under a pressure of 3.5 *** show that by compositing with 7 mol%Ag_(2)Te,the Seebeck coefficient of Cr_(1-x)Te is largely increased while the lattice thermal conductivity is considerably reduced,leading to 72%improvement of *** comparison,-△S_(M)is only slightly reduced by 10%in the *** work demonstrates the potential of Cr_(1-x)Te/Ag_(2)Te composites for thermoelectromagnetic cooling.

关键词： thermoelectromagnetic cooling thermoelectric magnetocaloric composite chromium telluride

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Ablation resistance of ZrC coating modified by polymer-derived SiHfOC ceramic microspheres at ultrahigh temperature

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Journal of materials Science & technology 2024年第15期182卷 119-131页

作者： Xuemeng Zhang Yuyu Zhang Lingxiang Guo Bing Liu Yuqi Wang Hongbin Li Hejun Li Jia Sun Shaanxi Key Laboratory of Fiber Reinforced Light Composite Materials State Key Laboratory of Solidification ProcessingNorthwestern Polytechnical UniversityXi’an 710072China China Aerodynamics Research and Development Center Mianyang 621000China Science and Technology on Advanced Ceramic Fibers and Composites Laboratory National University of Defense TechnologyChangsha 410073China

Polymer-derived ceramics(PDCs)method opens up new possibilities for the preparation of novel multi-phase ceramic nanocomposites owing to the molecular design of the precursors at the nanoscale *** the current work,ZrC coatings incorporated with polymer-derived ceramic microspheres(CMS),SiH-fOC_CMS,were deposited to enhance the ablation resistance by supersonic atmosphere plasma *** 10.0 MW·m^(-2) plasma ablation at above 3000℃,the linear ablation rate of ZrC-SiHfOC_CMS coat-ing was reduced to 0.20μm·s^(-1),62%lower than that of the pristine ZrC *** improvement was ascribed to the presentence of viscous SiO_(2)/HfO_(2) molten mixed phase,rather than HfSiO4,which can ef-fectively seal pinholes and ***,the in-situ generated crystalline SiO_(2) had a lower oxygen diffusion rate than amorphous SiO_(2),meanwhile,m-HfO_(2) could improve the stability of SiO_(2) glassy film,thus further enhancing the ablation resistance.

关键词： ZrC Polymer-derived ceramics(PDCs) Carbon/Carbon composites Plasma spraying Plasma ablation

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High performance wide bandgap perovskite solar cell with low V_(OC) deficit less than 0.4 V

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Journal of Energy Chemistry 2024年第4期91卷 313-322页

作者： Haikuo Guo Fuhua Hou Xuli Ning Xiaoqi Ren Haoran Yang Rui Liu Tiantian Li Chengjun Zhu Ying Zhao Wei Li Xiaodan Zhang School of Physical Science and Technology Key Laboratory of Semiconductor Photovoltaic Technology and Energy Materials at Universities of Inner Mongolia Autonomous RegionInner Mongolia UniversityHohhot 010021Inner MongoliaChina Institute of Photoelectronic Thin Film Devices and Technology of Nankai University Key Laboratory of Photoelectronic Thin Film Devices and Technology of TianjinSolar Energy Research Center of Nankai UniversityTianjin 300350China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430000HubeiChina

Wide bandgap perovskite solar cells(PSCs)have attracted significant attention because they can be applied to the top cells of tandem solar ***,high open-circuit voltage(V_(OC))deficit(>0.4 V)result from poor crystallization and high non-radiative recombination losses become a serious limitation in the pursuit of high ***,the relevance between different Pbl_(2)proportions and performance parameters are revealed through analysis of surface morphology,residual stress,and *** increase of Pbl_(2)proportion promotes crystal growth and reduces the work function of the perovskite film surface and promotes the energy level alignment with the carrier transport layer,which decreased the V_(OC)***,residual PbI_(2)exacerbated the stress level of perovskite film,and the resulting lattice disorder deteriorated the photostability of the ***,after the synergistic passivation of residual PbI_(2)and PEAI,the V_(OC)achieves 1.266 V and V_(OC)deficit is less than 0.4 V,the record value in wide bandgap PSCs.

关键词： Pb management Perovskite solar cell Strain Wide bandgap Stability

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Nanopore-rich NiFe LDH targets the formation of the high-valent nickel for enhanced oxygen evolution reaction

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Nano Research 2023年第2期16卷 2286-2293页

作者： Qunlei Wen Shuzhe Wang Ruiwen Wang Danji Huang Jiakun Fang Youwen Liu Tianyou Zhai State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China State Key Lab of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Nickel-iron layered double hydroxides(NiFe LDHs)represent a promising candidate for oxygen evolution reaction(OER),however,are still confronted with insufficient activity,due to the slow kinetics of electrooxidation of Ni^(2+)cations for the high-valent active ***,nanopore-rich NiFe LDH(PR-NiFe LDH)nanosheets were proposed for enhancing the OER activity together with *** the designed catalyst,the confined nanopores create abundant unsaturated Ni sites at edges,and decrease the migration distance of protons down to the scale of their mean free path,thus promoting the formation of high-valent Ni^(3+)/^(4+)active *** unique configuration further improves the OER stability by releasing the lattice stress and accelerating the neutralization of the local acidity during the phase ***,the optimized PR-NiFe LDH catalysts exhibit an ultralow overpotential of 278 mV at 10 mA∙cm^(−2)and a small Tafel slope of 75 mV∙dec^(−1),which are competitive among the advanced LDHs based ***,the RP-NiFe LDH catalyst was implemented in anion exchange membrane(AEM)water electrolyzer devices and operated steadily at a high catalytic current of 2 A over 80 *** results demonstrated that PR-NiFe LDH could be a viable candidate for the practical *** concept also provides valuable insights into the design of other catalysts for OER and beyond.

关键词： nickel-iron layered double hydroxides(NiFe LDHs) water oxidation nanopores high-valent sites

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Vertically mounting molybdenum disulfide nanosheets on dimolybdenum carbide nanomeshes enables efficient hydrogen evolution

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Nano Research 2022年第5期15卷 3946-3951页

作者： Tingting Wang Pengyan Wang Yajun Pang Yitian Wu Jin Yang Hao Chen Xiaorui Gao Shichun Mu Zongkui Kou State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China College of Chemistry and Materials Engineering Zhejiang A&F UniversityHangzhou 311300China Jiangsu Laboratory of Advanced Functional Materials School of Electronic and Information EngineeringChangshu Institute of TechnologyChangshu 215500China

Designing hierarchical heterostructure to optimize the adsorption of hydrogen intermediate(H*)is impressive for hydrogen evolution reaction(HER)***,we show that vertically mounting two-dimensional(2D)layered molybdenum disulfide(MoS_(2))nanosheets on 2D nonlayered dimolybdenum carbide(Mo_(2)C)nanomeshes to form a hierarchical heterostructure largely accelerates the HER kinetics in acidic electrolyte due to the weakening adsorption strength of H*on 2D Mo_(2)C *** hierarchical MoS2/Mo2C heterostructure therefore gives a decrease of overpotential for up to 500 mV at-10 mA·cm^(-2)and an almost 200-fold higher kinetics current density compared with the pristine Mo2C nanomeshes and maintains robust stability with a small drop of overpotential for only 16 mV upon 5,000 *** further rationalize this finding by theoretical calculations and find an optimized adsorption free energy of H*,identifying that the MoS_(2)featuring strong H*desorption plays a key role in weakening the strong binding of Mo_(2)C with H*and therefore improves the intrinsic HER activity on active C sites of Mo_(2)*** present finding shines the light on the rational design of heterostructured catalysts with synergistic geometry.

关键词： hydrogen evolution reaction transition metal carbide transition metal disulfide two-dimensional nonlayered/layered heterostructure hydrogen adsorption/desorption

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Coupling Co-Ni phosphides for energy-saving alkaline seawater splitting

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Nano Research 2024年第6期17卷 4797-4806页

作者： Weijia Liu Wenxian Liu Tong Hou Junyang Ding Zhigui Wang Ruilian Yin Xingyuan San Ligang Feng Jun Luo Xijun Liu State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Nonferrous Metals and Featured MaterialsMOE Key Laboratory of New Processing Technology for Nonferrous Metals and MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China Hebei Key Laboratory of Optic-electronic Information and Materials the College of Physics Science and TechnologyHebei UniversityBaoding 071002China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

The coupling of energy-saving small molecule conversion reactions and hydrogen evolution reaction(HER)in seawater electrolytes can reduce the energy consumption of seawater electrolysis and mitigate chlorine corrosion ***,the fabrication of efficient multifunctional catalysts for this promising technology is of great ***,a heterostructured catalyst comprising CoP and Ni_(2)P on nickel foam(CoP/Ni_(2)P@NF)is reported for hydrazine oxidation(HzOR)-assisted alkaline seawater *** coupling of CoP and Ni_(2)P optimizes the electronic structure of the active sites and endows excellent electrocatalytic performance for HzOR and ***,the two-electrode HzOR-assisted alkaline seawater splitting(OHzS)cell based on the CoP/Ni_(2)P@NF required only 0.108 V to deliver 100 mA·cm^(−2),much lower than 1.695 V for alkaline seawater electrolysis ***,the OHzS cell exhibits satisfactory stability over 48 h at a high current density of 500 mA·cm^(−2).Furthermore,the CoP/Ni_(2)P@NF heterostructured catalyst also efficiently catalyzed glucose oxidation,methanol oxidation,and urea oxidation in alkaline seawater *** work paves a path for high-performance heterostructured catalyst preparation for energy-saving seawater electrolysis for H_(2) production.

关键词： seawater splitting heterostructure electrocatalysis hydrazine oxidation reaction hydrogen evolution reaction

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Realizing Highly Reversible Zinc Anode via Controlled-current Pre-deposition

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Energy & Environmental materials 2023年第6期6卷 327-334页

作者： Xinghang Chen Ming Li Qi Li Yuzhu Chen Buke Wu Meng Lin Qinyou An Liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyHubeiWuhan 430070China Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong LaboratoryXianhu Hydrogen ValleyFoshan 528200China Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055China SUSTech Energy Institute for Carbon Neutrality Southern University of Science and TechnologyShenzhen China Shenzhen Key Laboratory of Advanced Energy Storage Southern University of Science and TechnologyShenzhen 518055China

Aqueous zinc ion batteries have been considered as the prominent candidate in the next-generation batteries for its low cost,safety and high theoretical ***,formation of zinc dendrites and side reactions at the electrode/electrolyte interface during the zinc plating/stripping process affect the cycling reversibility of the zinc *** of the zinc plating/stripping process and realizing a highly reversible zinc anode is a great ***,we applied a simple and effective approach of controlled-current zinc pre-deposition at copper *** the current density of 40 mA cm^(-2),where the electron/ion transfers are both continuous and balanced,the Zn@CM-40 electrode with the(002)crystal plane orientation and the compactly aligned platelet morphology was successfully *** with the zinc foil,the Zn@CM-40 exhibits greatly enhanced reversibility in the repeated plating/stripping(850 h at 1 mA cm^(-2))for the symmetric battery test.A series of characterization techniques including electrochemical analyses,XRD,SEM and optical microscopy observation,were used to demonstrate the correlation between the structure of pre-deposited zinc layer and the cycling *** COSMOL Multiphysics modeling demonstrates a more uniform electric field distribution in the Zn@CM than the zinc foil due to the aligned platelet ***,the significant improvement is also achieved in a Zn||MnO_(2)full battery with a high capacity-retention(87%vs 47.8%).This study demonstrates that controlled-current electrodeposition represents an important strategy to regulate the crystal plane orientation and the morphology of the pre-deposited zinc layer,hence leading to the highly reversible and dendrite-free zinc anode for high-performance zinc ion batteries.

关键词： controlled-current pre-deposition dendrite-free reversible zinc anode zinc ion battery

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Highly Selective Photocatalytic Conversion of Glucose on Holo-Symmetrically Spherical Three-Dimensionally Ordered Macroporous Heterojunction Photonic Crystal

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CCS Chemistry 2023年第8期5卷 1773-1788页

作者： Ting-Wei Wang Zhi-Wen Yin Yin-Hao Guo Fang-Yuan Bai Jun Chen Wenda Dong Jing Liu Zhi-Yi Hu Lihua Chen Yu Li Bao-Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology430070 Wuhan Nanostructure Research Centre(NRC) Wuhan University of Technology430070 Wuhan Laboratory of Inorganic Materials Chemistry(CMI) University of NamurB-5000 Namur

Photocatalytic conversion of biomass is considered an effective,clean,and environmentally friendly route to obtain high-valued chemicals and ***,the limited conversion efficiency and poor selectivity are still the main bottlenecks for photocatalytic biomass ***,we report the highly selective photocatalytic conversion of glucose solution on holosymmetrically spherical three-dimensionally ordered macroporous TiO_(2)-CdSe heterojunction photonic crystal structure(s-TCS).The obtained s-TCS photocatalysts show excellent stability and strong light harvesting,uniform mass diffusion and exchange,and efficient photogenerated electrons/holes separation and *** optimized s-TCS-4 photocatalyst displays the highest photocatalytic performance for glucose oxidation and hydrogen *** glucose conversion,lactic acid selectivity,and yield on s-TCS-4 are about 95.9%,94.3%,and 96.4%,*** photocatalytic production of lactic acid for s-TCS-4(18.5 g/L)is 2.3 times higher than the pure spherical TiO_(2) photonic crystal without CdSe(s-TiO_(2),8.1 g/L),and the hydrogen production rate of s-TCS-4 is 9.4 times that of s-TiO_(2).For the first time,we reveal that the photocatalytic conversion of glucose to lactic acid is a third-order and four-electron-involved *** work could shed some new light on the efficient photocatalysis conversion of biomass to highly value-added products with high selectivity and yield,and simultaneously sustainable hydrogen evolution.

关键词： TiO_(2)-CdSe heterojunction spherical photonic crystal high-selective photocatalytic glucose conversion lactic acid photocatalytic H2 production four-electron involved reaction third-order reaction

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High-rate sodium-ion storage of vanadium nitride via surface-redox pseudocapacitance

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Interdisciplinary materials 2023年第3期2卷 434-442页

作者： Qiulong Wei Tingyi Huang Xiaojuan Huang Binhao Wang Yalong Jiang Dafu Tang Dong-Liang Peng Bruce Dunn Liqiang Mai Department of Materials Science and Engineering Fujian Key Laboratory of Surface and Interface Engineering for High Performance MaterialsCollege of MaterialsXiamen UniversityXiamenChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanChina Department of Materials Science and Engineering University of California Los AngelesLos AngelesCaliforniaUSA

Vanadium nitride(VN)electrode displays high-rate,pseudocapacitive responses in aqueous electrolytes,however,it remains largely unclear in nonaqueous,Na+-based *** traditional view supposes a conversion-type mechanism for Na+storage in VN anodes but does not explain the phenomena of their size-dependent specific capacities and underlying causes of pseudocapacitive charge storage ***,we insightfully reveal the VN anode exhibits a surface-redox pseudocapacitive mechanism in nonaqueous,Na+-based electrolytes,as demonstrated by kinetics analysis,experimental observations,and first-principles *** ex situ X-ray photoelectron spectroscopy and semiquantitative analyses,the Na+storage is characterized by redox reactions occurring with the V5+/V4+to V3+at the surface of VN particles,which is different from the well-known conversion reaction *** pseudocapacitive performance is enhanced through nanoarchitecture design via oxidized vanadium states at the *** optimized VN-10 nm anode delivers a sodium-ion storage capability of 106 mAh g−1 at the high specific current of 20 A g−1,and excellent cycling performance of 5000 cycles with negligible capacity *** work demonstrates the emerging opportunities of utilizing pseudocapacitive charge storage for realizing high-rate sodium-ion storage applications.

关键词： high-rate capability pseudocapacitance sodium-ion storage vanadium nitride

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